CN104479738B - A kind of Deep Desulfurization of FCC Gasoline combination process - Google Patents
A kind of Deep Desulfurization of FCC Gasoline combination process Download PDFInfo
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- CN104479738B CN104479738B CN201410781964.4A CN201410781964A CN104479738B CN 104479738 B CN104479738 B CN 104479738B CN 201410781964 A CN201410781964 A CN 201410781964A CN 104479738 B CN104479738 B CN 104479738B
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G67/00—Treatment of hydrocarbon oils by at least one hydrotreatment process and at least one process for refining in the absence of hydrogen only
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2400/00—Products obtained by processes covered by groups C10G9/00 - C10G69/14
- C10G2400/02—Gasoline
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Abstract
The present invention relates to a kind of method for Deep Desulfurization of FCC Gasoline, comprising: first paragraph reaction is thioetherification reaction; After reaction, gasoline is cut into weight two portions by rectifying tower; Second segment reaction is heavy constituent selective hydrodesulfurization and isomerization; 3rd section of reaction is the hydrodesulfurization process of secondary mercaptan after selective hydrodesulfurization process; 4th section of reaction is Etherification of Light FCC Gasoline; Finally light, biharmonic obtains the super low-sulfur oil product meeting state V gasoline quality standard.This invention is applicable to the hydro-upgrading of catalytically cracked gasoline, and desulfurization degree is high, and liquid yield is high, and each unit catalyst stability is good, the life-span is long, and whole process is discharged without alkaline residue.
Description
Technical field
The present invention relates to a kind of method of producing clean gasoline product; More specifically, a kind of method of Deep Desulfurization of FCC Gasoline is related to.
Background technology
Along with increasingly sharpening of topsoil, various countries are to the NO in Motor vehicles discharging waste gas
x, SO
xpropose harsher restriction with aromaticity content etc., especially China in recent years northern each metropolitan haze weather impel country to improve further the specifications of quality requirement of fuel oil for vehicles.For motor spirit, China implements the state IV gasoline standard of sulphur content lower than 50ppm in January, 2014, and plan in January, 2018 whole nation carry out sulphur content lower than the state V gasoline standard of 10ppm, and the big city headed by Beijing, Shanghai has taken the lead in state of enforcement V gasoline standard.Therefore, factory of domestic each great oil refining faces the task of severe quality of gasoline upgrading.
But the hydrogenating desulfurization technology of Most current refinery, to improve the severity of processing conditions further, exists alkene saturated in a large number, directly causes octane value significantly to lose, hydrogen consumption increases, the defect that oil quality declines.In recent years, China Petrochemical Industry system refinery is introduced and through the S-Zorb adsorption desulfurize technology of autonomous innovation, although the sulphur content in oil product can be reduced to below 10ppm, but due in gasoline containing a large amount of alkene, diolefine and colloid and other non-persistent compound, cause gasoline stability poor.PetroChina Company Limited. and China University Of Petroleum Beijing develop the selective hydrodesulfurization technology DSO technique and GARDES technique that meet producing country V normal benzene, by segmentation desulfurization and octane value recovering technology, obtain higher desulfurization degree and liquid yield, but still there is the problem of loss of octane number.
Patent CN201110321289.3 discloses a kind of processing method of producing ultra-clean gasoline.Catalytically cracked gasoline enters hydrogenation preliminary fractionator and fractionates out gasoline lighting end and last running, and lighting end is fixed an oxidation deodorizing, and mercaptan is converted into disulphide, and deodorization product mixes with thermocatalysis diesel oil and fractionates out lighting end and diesel oil distillate through separation column; Catalytically cracked gasoline last running carries out hydrogenating desulfurization through high reactivity/low activity combined hydrogenation catalyzer, and after desulfurization product and deodorization, lighting end is mixed to get clean gasoline product.Compared with prior art, the sulphur content of catalytically cracked gasoline can be reduced to 10 below μ g/g by this inventive method, and loss of octane number is few, and mercaptans content is qualified; The colloid generated in deodorising process can be avoided to enter last running selective hydrogenation unit simultaneously, avoid hydrogenation unit pressure drop to produce, prolong operating period.
Patent CN201310256949.3 discloses a kind of method for modifying of catalytic gasoline of whole fraction.Catalytic gasoline of whole fraction raw material enters pre-hydroprocessing unit and removes diolefine.Effluent enters selective hydrodesulfurization treatment reactor, after Hydrobon catalyst contact reacts, enters octane value recovering reactor, and with octane value recovering catalyst contact reacts, effluent obtains the upgraded products of low sulfur-bearing after gas-liquid separation.This invention carries out hydrogenating desulfurization and octane value recovering process by catalytic gasoline of whole fraction total sulfur content being less than to 400ppm, and upgraded products sulphur content is down to below 50ppm, and loss of octane number is less than a unit simultaneously.
Patent CN201010584150.3 discloses a kind of efficient combination production method of ultra-low sulfur and high-octane number gasoline.This production method comprises: make full distillation gasoline raw material inferior under hydro condition, carry out the directed sulphur shift reaction of low temperature, then carry out oil product cutting fractionation, obtain lighting end gasoline and last running gasoline, cutting cut point is 50-90 DEG C; Make last running gasoline and catalyst for selectively hydrodesulfurizing and supplementary desulfurization-hydro carbons isomery/aromatization catalyst exposure; By the last running gasoline mixing after lighting end gasoline and process, obtain the gasoline products of ultra-low sulfur and high-octane number.This invention is applicable to the upgrading of inferior patrol, especially can obtain good ultra-deep desulfurization, Olefin decrease effect to the catalytically cracked gasoline inferior of ultra-high-sulfur(UHS), high olefin, and can maintain or improve the octane value of product after reaction and keep higher product yield.
Patent CN201310473031.4 discloses the process integration of a kind of catalytic gasoline selective hydrogenation technique and Etherification of Light FCC Gasoline, combining of catalytic gasoline selective hydrogenation and Etherification of Light FCC Gasoline two technological process novelties is integrated by this technique, sulphur is removed by process for selective hydrogenation, nitrogen etc., its isolated light oil constituents Tertiary olefin content is high, again by generating tert-pentyl ethers with the etherification reaction of methyl alcohol, thus effectively reduce the olefin(e) centent of petroleum naphtha component, increase petroleum naphtha octane value, its medium sulphide content decreasing ratio is greater than 90%, diolefine removes substantially completely, in addition, after etherificate unit, octane value can improve 2 ~ 6 units.
But the gasoline hydrodesulfurizationmethod technology in above-mentioned patent mainly adopts the mode of two or more Combination of Methods of segmentation desulfurization, selective hydrodesulfurization and octane value recovering etc. to reach deep desulfuration, avoids loss of octane number simultaneously.But it is comparatively large still to there is loss of octane number in these methods, and secondary Mercaptan removal does not thoroughly cause desulfurization degree to decline, or product liquid receives the shortcomings such as lower.
Summary of the invention
The object of this invention is to provide a kind of method of Deep Desulfurization of FCC Gasoline.The method is mainly according to different hydrocarbons composition and the sulphidic species distribution of catalytically cracked gasoline, by mercaptan etherification technology, cutting weight component, the hydrogenating desulfurization of heavy constituent depth-selectiveness and straight chain hydrocarbon isomerization recover octane value, secondary Mercaptan removal and Etherification of Light FCC Gasoline and improve the process optimization combinations such as gasoline octane rating, refining catalytic gasoline desulfurization improves the octane value of gasoline simultaneously, the quality of improving product, reaches the requirement of production high-quality state V normal benzene.
The method of Deep Desulfurization of FCC Gasoline of the present invention mainly comprises four sections of simple reaction process and a rectification process catalytically cracked gasoline, wherein first paragraph reaction is thioetherification reaction unit, second segment reacts attach most importance to compositional selecting hydrogenating desulfurization and isomerization reaction unit, 3rd section of reaction is the hydrodesulfurization process of selective hydrodesulfurization process secondary mercaptan, and the 4th section of reaction is Etherification of Light FCC Gasoline reaction process.After first paragraph reaction, through a rectification process, catalytically cracked gasoline is cut into weight two portions.Finally light, biharmonic obtains the ultra-low sulfur gasoline products after refining.Specifically, the method comprises the following steps:
(1) enter mercaptan etherification reaction tower after being mixed with a certain amount of hydrogen by catalytically cracked gasoline, under catalyst action, the thioetherification reaction of mercaptan and alkene or diolefine occurs, diolefine is hydrogenated to monoolefine by selectivity simultaneously;
(2) gasoline that step (1) obtains is cut into gently by rectifying tower, heavy constituent, and light constituent is the light gasoline fraction being rich in alkene of not sulfur-bearing, and restructuring is divided into is rich in sulphur and the less heavy naphtha of alkene;
(3) heavy naphtha that step (2) obtains enters the selective hydrodesulfurization tower of filling catalyst for selectively hydrodesulfurizing and isomerization catalyst, carries out the hydrogenating desulfurization of the degree of depth and the isomerization reaction of straight chain hydrocarbon;
(4) heavy naphtha that obtains of step (3) is by secondary mercaptan hydrogenation and removing tower, secondary mercaptan in removing gasoline, thus obtains the heavy naphtha through deep desulfuration purification;
(5) the Etherification of Light FCC Gasoline reaction tower loading acidic etherification catalysts is entered after the light gasoline fraction that obtains of step (2) and a certain amount of methanol mixed, by high-octane for the conversion of olefines in light gasoline fraction ether compound, reduce olefin(e) centent simultaneously;
(6) the light gasoline fraction mixing that obtains of the heavy naphtha that obtains of step (4) and step (5), obtains super low sulfur, clean gasoline product that octane value is high.
The mercaptan etherification reaction catalyzer of step (1) is the NiO/MgO-Al of Mo or W modification
2o
3catalyzer, described catalyzer needs to carry out prevulcanized process before the reaction.
Thioetherification reaction condition is: reaction pressure 0.5-3.5MPa, temperature 60-180 DEG C, air speed 1-10h
-1, hydrogen to oil volume ratio 0.5-20.
The cutting temperature that is light, heavy constituent of step (2) is 65 DEG C.
The selective hydrodesulfurization catalysts of step (3) is La
2o
3the Co-Mo/Al of modification
2o
3catalyzer, isomerization catalyst is Mo-Ni/SAPO-11-ZSM-5 catalyzer, and two class catalyzer need to carry out prevulcanized process before the reaction.
The processing condition of selective hydrodesulfurization and isomerization reaction are: reaction pressure 0.5-3.5MPa, temperature 200-320 DEG C, air speed 1-10h
-1, hydrogen to oil volume ratio 50-200.
The catalyzer of the secondary mercaptan hydrogenation and removing of step (4) is Mo (W)-Ni (Co)/Al
2o
3catalyzer, described catalyzer needs to carry out prevulcanized process before the reaction.
The processing condition of secondary Mercaptan removal are: reaction pressure 0.1-2MPa, temperature 100-220 DEG C, air speed 1-10h
-1, hydrogen to oil volume ratio 10-100.
The acidic etherification catalysts of step (5) is selected from acid sulfonic resin, heteropolyacid, solid super-strong acid, molecular sieve.
The processing condition of acidic etherification reaction are: reaction pressure 0.1-2MPa, temperature 40-120 DEG C, air speed 1-10h
-1.
Compared with prior art, the method for Deep Desulfurization of FCC Gasoline of the present invention has following beneficial effect:
(1) simply, desulfurization depth is high for this technological process principle and flow process, and each unit catalyzer is ripe, the life-span is long, is extensively applicable to the fine de-sulfur process that refinery utilizes catalytically cracked gasoline producing country V normal benzene;
(2) desulfurization degree is high, Sulfur Content in Catalytic Cracking Gasoline can be down to 10 below μ g/g; Liquid yield is high, and can improve 1-6 unit after the process of product octane value.
Accompanying drawing explanation
Fig. 1 is process flow sheet of the present invention.Wherein, A is catalytically cracked gasoline raw material, and B, C and D are hydrogen, and E is methyl alcohol, and F is high-octane rating low-sulphur oil.1 is thioetherification reaction tower, and 2 is rectifying tower, and 3 is difunctional selective hydrodesulfurization reaction tower, 4 two mercaptan hydrogenation and removing reaction towers, and 5 is light oil etherification reaction tower.
Embodiment
Further illustrate preparation method of the present invention as embodiment below, will contribute to further understanding of the invention, protection scope of the present invention is not limited to the examples, and its protection domain is decided by claims.
Embodiment 1
The fixed-bed reactor 1 loading mercaptan etherification reaction catalyzer are entered after full cut catalytic cracking stable gasoline raw material A mixes with hydrogen B, at reaction pressure 0.5-3.5MPa, temperature 60-180 DEG C, air speed 1-10h
-1, under hydrogen to oil volume ratio 0.5-20 condition, mercaptan and alkene or diolefine generation thioetherification reaction, be converted into heavy thioether by mercaptan, and diolefine is hydrogenated to monoolefine by selectivity simultaneously.After reaction, gasoline enters a rectifying tower and full distillation gasoline is cut into weight two portions, and wherein cut point temperature is 65 DEG C, and tower top is be rich in the petroleum naphtha component of alkene without sulphur.Last running at the bottom of tower mixes laggard selectable hydrogenator with hydrogen C, at reaction pressure 0.5-3.5MPa, and temperature 200-320 DEG C, air speed 1-10h
-1, carry out depth-selectiveness hydrogenating desulfurization and isomerization reaction under hydrogen to oil volume ratio 50-200 condition, to heavy gasoline components desulfurization and recuperation section octane value.Containing the secondary mercaptan that hydrodesulfurization process is formed in gasoline after selective hydrodesulfurization, after mixing with hydrogen D, enter secondary mercaptan hydrogenating desulfurization tower again, at reaction pressure 0.1-2MPa, temperature 100-220 DEG C, air speed 1-10h
-1, hydro-sweetening under the mitigation condition of hydrogen to oil volume ratio 10-100.By loading a kind of reactor of catalyzer of acid sulfonic resin, heteropolyacid, solid super-strong acid, molecular sieve after the mixing with a certain amount of methyl alcohol E without sulphur light constituent of what rectifying tower top obtained be rich in alkene, at reaction pressure 0.1-2MPa, temperature 40-120 DEG C, air speed 1-10h
-1carry out etherification reaction under condition, reduce olefin(e) centent in gasoline, and improve octane value.Finally, light, weigh two components and be mixed to get super low sulfur, high-octane gasoline products F.
Table 1 is the Deep Desulfurization of FCC Gasoline refining effect correlative value through process for purification process of the present invention under different technology conditions.The gasoline products of different sulphur contents can be produced by controlling different processing condition by table 1, wherein first scheme gasoline index after deep desulfuration meets state IV standards requirement, and octane value can improve 2.9 units, second and third scheme can be produced and be met state V normal benzene, and octane value also can improve more than a nearly unit.
Catalytically cracked gasoline sweetening effectiveness contrast under table 1 different condition
Can find out, method of the present invention has that low, each unit catalyst stability of cost of investment is good, the life-span is long, product desulfurization degree is high, quality better, the omnidistance advantage without alkaline residue discharge etc.
Claims (9)
1., for a method for Deep Desulfurization of FCC Gasoline, comprise the following steps:
(1) enter mercaptan etherification reaction tower after being mixed with a certain amount of hydrogen by catalytically cracked gasoline, under catalyst action, the thioetherification reaction of mercaptan and alkene or diolefine occurs, diolefine is hydrogenated to monoolefine by selectivity simultaneously;
(2) gasoline that step (1) obtains is cut into gently by rectifying tower, heavy constituent, and light constituent is the light gasoline fraction being rich in alkene of not sulfur-bearing, and restructuring is divided into is rich in sulphur and the less heavy naphtha of alkene; The cutting temperature that is light, heavy constituent of wherein said step (2) is 65 DEG C;
(3) heavy naphtha that step (2) obtains enters the selective hydrodesulfurization tower of filling catalyst for selectively hydrodesulfurizing and isomerization catalyst, carries out the hydrogenating desulfurization of the degree of depth and the isomerization reaction of side chain hydro carbons;
(4) heavy naphtha that obtains of step (3) is by secondary mercaptan hydrogenation and removing tower, secondary mercaptan in removing gasoline, thus obtains the heavy naphtha through deep desulfuration purification;
(5) the Etherification of Light FCC Gasoline reaction tower loading acidic etherification catalysts is entered after the light gasoline fraction that obtains of step (2) and a certain amount of methanol mixed, by high-octane for the conversion of olefines in light gasoline fraction ether compound, reduce olefin(e) centent simultaneously;
(6) the light gasoline fraction mixing that obtains of the heavy naphtha that obtains of step (4) and step (5), obtains super low sulfur, clean gasoline product that octane value is high.
2. method according to claim 1, the mercaptan etherification reaction catalyzer of wherein said step (1) is the NiO/MgO-Al of Mo or W modification
2o
3catalyzer, described catalyzer needs to carry out prevulcanized process before the reaction.
3. method according to claim 1 and 2, wherein said thioetherification reaction condition is: reaction pressure 0.5-3.5MPa, temperature 60-180 DEG C, air speed 1-10h
-1, hydrogen to oil volume ratio 0.5-20.
4. method according to claim 1, the selective hydrodesulfurization catalysts of wherein said step (3) is La
2o
3the Co-Mo/Al of modification
2o
3catalyzer, isomerization catalyst is Mo-Ni/SAPO-11-ZSM-5 catalyzer, and two class catalyzer need to carry out prevulcanized process before the reaction.
5. the method according to claim 1 or 4, the processing condition of wherein selective hydrodesulfurization and isomerization reaction are: reaction pressure 0.5-3.5MPa, temperature 200-320 DEG C, air speed 1-10h
-1, hydrogen to oil volume ratio 50-200.
6. method according to claim 1, the catalyzer of the secondary mercaptan hydrogenation and removing of wherein said step (4) is Mo (W)-Ni (Co)/Al
2o
3catalyzer, described catalyzer needs to carry out prevulcanized process before the reaction.
7. the method according to claim 1 or 6, the processing condition of wherein said secondary Mercaptan removal are: reaction pressure 0.1-2MPa, temperature 100-220 DEG C, air speed 1-10h
-1, hydrogen to oil volume ratio 10-100.
8. method according to claim 1, the acidic etherification catalysts of wherein said step (5) is selected from acid sulfonic resin, heteropolyacid, solid super-strong acid, molecular sieve.
9. the method according to claim 1 or 8, the processing condition of wherein said acidic etherification reaction are: reaction pressure 0.1-2MPa, temperature 40-120 DEG C, air speed 1-10h
-1.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| RU2742646C2 (en) * | 2016-10-21 | 2021-02-09 | Чайна Петролеум Энд Кемикал Корпорейшн | Method of gasoline treatment |
| RU2754030C2 (en) * | 2016-10-21 | 2021-08-25 | Чайна Петролеум Энд Кемикал Корпорейшн | Method for purifying gasoline |
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| CN107916130B (en) * | 2016-10-10 | 2019-08-06 | 中国石油化工股份有限公司 | The method of mercaptan thioetherification |
| CN107974293B (en) * | 2016-10-21 | 2020-06-16 | 中国石油化工股份有限公司 | Gasoline treatment method and system |
| CN107974295B (en) * | 2016-10-21 | 2020-03-24 | 中国石油化工股份有限公司 | Gasoline treatment method |
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| CN107974296B (en) * | 2016-10-21 | 2020-01-10 | 中国石油化工股份有限公司 | Gasoline treatment method |
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| CN107974291B (en) * | 2016-10-21 | 2019-10-25 | 中国石油化工股份有限公司 | A kind of processing method and system of gasoline |
| CN107974297B (en) * | 2016-10-21 | 2020-01-10 | 中国石油化工股份有限公司 | Gasoline treatment method |
| CN107974290B (en) * | 2016-10-21 | 2019-10-25 | 中国石油化工股份有限公司 | A kind of vapour oil treatment process |
| CN107974292B (en) * | 2016-10-21 | 2019-10-25 | 中国石油化工股份有限公司 | A kind of vapour oil treatment process |
| CN106635156B (en) * | 2016-12-26 | 2018-07-13 | 中国石油大学(北京) | A kind of method of Deep Desulfurization of FCC Gasoline |
| CN108949228B (en) * | 2017-05-19 | 2020-10-27 | 中国石油化工股份有限公司 | Method and system for producing clean gasoline |
| CN113122326B (en) * | 2020-01-15 | 2023-04-07 | 中国石油天然气股份有限公司 | Deep desulfurization method for full-fraction catalytic cracking gasoline |
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